Synthesis of novel LaCoO3/graphene catalysts as highly efficient peroxymonosulfate activator for the degradation of organic pollutants

被引:37
作者
Hammad, Mohaned [1 ]
Angel, Steven [4 ]
Al-Kamal, Ahmed K. [4 ,8 ]
Asghar, Anam [2 ,3 ]
Amin, Amin Said [1 ]
Kraeenbring, Mena-Alexander [1 ]
Wiedemann, Haakon T. A. [5 ]
Vinayakumar, Vineetha [1 ]
Ali, Md Yusuf [4 ]
Fortugno, Paolo [4 ]
Kim, Cheolyong [2 ,3 ]
Schmidt, Torsten C. [2 ,3 ]
Kay, Christopher W. M. [5 ,7 ]
Schulz, Christof [4 ,6 ]
Segets, Doris [1 ,6 ]
Wiggers, Hartmut [4 ,6 ]
机构
[1] Univ Duisburg Essen, Inst Combust & Gas Dynam Particle Sci & Technol I, Duisburg, Germany
[2] Univ Duisburg Essen, Instrumental Analyt Chem, Essen, Germany
[3] Univ Duisburg Essen, Ctr Water & Environm Res, Essen, Germany
[4] Univ Duisburg Essen, Inst Combust & Gas Dynam React Fluids IVG RF, Duisburg, Germany
[5] Saarland Univ, Dept Chem, Saarbrucken, Germany
[6] Univ Duisburg Essen, Ctr Nanointegrat Duisburg Essen CENIDE, Duisburg, Germany
[7] UCL, London Ctr Nanotechnol, 17-19 Gordon St, London WC1H 0AH, England
[8] Univ Al Mustansiriyah, Dept Mat Engn, Baghdad, Iraq
关键词
Bisphenol A; Gas-phase synthesis; Graphene; Heterogeneous catalysis; Peroxymonosulfate; BISPHENOL-A; SINGLET OXYGEN; HYDROTHERMAL SYNTHESIS; SULFATE RADICALS; GRAPHENE; REMOVAL; LACOO3; OXIDATION; WATER; COMPOSITE;
D O I
10.1016/j.cej.2022.139900
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Metal leaching in perovskite-based catalysts during peroxymonosulfate activation processes can severely restrict their application in wastewater treatment. Therefore, enhancing the stability of perovskite nanostructures is crucial to improve catalytic performance and broaden applications but has been rarely achieved so far. We developed a scalable method to synthesize novel stable and environmentally-friendly nanocomposites of LaCoO3 and few-layer graphene (consisting of roughly-nine layers) for the removal of organic pollutants from wastewater. With abundant oxygen vacancies and synergistic effects between LaCoO3 and few-layer graphene, the novel LaCoO3/graphene catalyst exhibits outstanding catalytic degradation (>99 %) of diclofenac, metoprolol, carbamazepine, and bisphenol A at a high concentration (40 mg/1) in less than 10 min in the peroxymonosulfate activation system, with mineralization of 57, 55, 61, and 62 %, respectively. The LaCoO3/graphene catalyst exhibited excellent reusability and high catalytic performance within a wide pH range (3-11). The formation of LaCoO3/graphene composites prevents cobalt leaching (0.004 mg/l), stabilizes sub-stoichiometric LaCoO3 and thus increases the content of Co2+ in the structure, leading to much higher catalytic activity than that of pure LaCoO3. Electron paramagnetic resonance and radical quenching experiments revealed that both radical pathways (SO4 center dot-, (OH)-O-center dot, and O-2(center dot-)) and non-radical pathways (O-1(2)) contribute to bisphenol A degradation and the relative contributions of (OH)-O-center dot, SO4 center dot-, and O-1(2)/O-2(center dot-) were determined to 13.4, 32.6, and 54 % for bisphenol A removal, respectively. Overall, our results indicate that LaCoO3/graphene is a promising material towards peroxymonosulfate activation for environmental remediation.
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页数:16
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共 104 条
[41]   Graphene encapsulated FexCoy nanocages derived from metal-organic frameworks as efficient activators for peroxymonosulfate [J].
Li, Xuning ;
Rykov, Alexandre I. ;
Zhang, Bo ;
Zhang, Yanjie ;
Wang, Junhu .
CATALYSIS SCIENCE & TECHNOLOGY, 2016, 6 (20) :7486-7494
[42]   Simultaneous oxidation of 4-aminophenylarsonic acid and adsorption of the produced inorganic arsenic by a combination of Co3O4-La2CO5@RSBC with peroxymonosulfate [J].
Li, Yuxin ;
Liu, Li ;
Wang, Zeming ;
Zhou, Lixiang ;
Lan, Yeqing ;
Chen, Cheng .
CHEMICAL ENGINEERING JOURNAL, 2021, 413
[43]   Synthesis of novel Co3O4 hierarchical porous nanosheets via corn stem and MOF-Co templates for efficient oxytetracycline degradation by peroxymonosulfate activation [J].
Li, Zhilin ;
Wang, Min ;
Jin, Chongyue ;
Kang, Jin ;
Liu, Jun ;
Yang, Hairong ;
Zhang, Yueqiu ;
Pu, Qianyun ;
Zhao, Yu ;
You, Meiyan ;
Wu, Zengmin .
CHEMICAL ENGINEERING JOURNAL, 2020, 392
[44]   A rapid spectrophotometric determination of persulfate anion in ISCO [J].
Liang, Chenju ;
Huang, Chiu-Fen ;
Mohanty, Nihar ;
Kurakalva, Rama Mohan .
CHEMOSPHERE, 2008, 73 (09) :1540-1543
[45]   Cation deficiency tuned LaCoO3-δ perovskite for peroxymonosulfate activation towards bisphenol A degradation [J].
Liang, Ping ;
Meng, Dingding ;
Liang, Yi ;
Wang, Zheng ;
Zhang, Chi ;
Wang, Shaobin ;
Zhang, Zhonghua .
CHEMICAL ENGINEERING JOURNAL, 2021, 409
[46]   Efficient adsorption and sustainable degradation of gaseous acetaldehyde and o-xylene using rGO-TiO2 photocatalyst [J].
Lin, Wenjiao ;
Xie, Xiaofeng ;
Wang, Xiao ;
Wang, Yan ;
Segets, Doris ;
Sun, Jing .
CHEMICAL ENGINEERING JOURNAL, 2018, 349 :708-718
[47]   Coupling metal-organic frameworks and g-C3N4 to derive Fe@N-doped graphene-like carbon for peroxymonosulfate activation: Upgrading framework stability and performance [J].
Liu, Chao ;
Liu, Liyuan ;
Tian, Xing ;
Wang, Yiping ;
Li, Ruoyu ;
Zhang, Yuting ;
Song, Zilong ;
Xu, Bingbing ;
Chu, Wei ;
Qi, Fei ;
Ikhlaq, Amir .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2019, 255
[48]   Strategies for chemical modification of graphene and applications of chemically modified graphene [J].
Liu, Jingquan ;
Tang, Jianguo ;
Gooding, J. Justin .
JOURNAL OF MATERIALS CHEMISTRY, 2012, 22 (25) :12435-12452
[49]   Simultaneous removal of NO and SO2 using vacuum ultraviolet light (VUV)/heat/peroxymonosulfate (PMS) [J].
Liu, Yangxian ;
Wang, Yan ;
Wang, Qian ;
Pan, Jianfeng ;
Zhang, Jun .
CHEMOSPHERE, 2018, 190 :431-441
[50]   Sandwich-like Co3O4/MXene composite with enhanced catalytic performance for Bisphenol A degradation [J].
Liu, Yuxin ;
Luo, Rui ;
Li, Yang ;
Qi, Junwen ;
Wang, Chaohai ;
Li, Jiansheng ;
Sun, Xiuyun ;
Wang, Lianjun .
CHEMICAL ENGINEERING JOURNAL, 2018, 347 :731-740